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Coupling of Chemical Processes in the Near Field

  • B. Grambow (a1) and E. Giffaut (a2)

Abstract

Coupled modelling has been performed using geochemical/transport codes and radiolysis models to describe the chemical evolution of the waste forms “high-level waste glass” and “spent nuclear fuel” together with its waste package and engineered barrier surroundings. Near field processes considered include container corrosion, hydrogen generation, mass transfer for radionuclides and other waste matrix components in corrosion products and buffer materials, geochemistry of near field solution chemistry, sorption of radionuclides on surface sites in the nano-sized pore space of near field materials and the radiolytic decomposition of pore water. The rate limiting steps in waste form dissolution and secondary phase formation mechanism and the associated radionuclide mobilisation chemistry (solubility, solid solution formation, speciation, redox stability) are strongly influenced by the near field constraints.

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1. Vernaz, E. et al. , Present understanding of R7T7 glass alteration kinetics and their impact on long-term alteration modeling. J. Nucl. Mater., 2001. 298 p. 2736.
2. Grambow, B. and Müller, R., First order dissolution rate law and the role of surface layers in glass performance assessment. J. Nucl. Mat., 2001. 298 p. 112124.
3. Ribet, I. et al. , GLASTAB, Long-term behaviour of glass: improving the glass source term and substantiating the basic hypotheses, CONTRACT N°FIKW-CT-2000-00007, FINAL TECHNICAL REPORT. 2004.
4. Advocat, T. et al. , Effect of geological repository parameters on aqueous corrosion of nuclear waste glass. 1996, European Commission: Luxemburg.
5. Ribet, S. 2005: Nantes.
6. Parkhurst, D.L. and Appelo, C.A.J., USER'S GUIDE TO PHREEQC (VERSION 2)- A COMPUTER PROGRAM FOR SPECIATION, BATCH-REACTION, ONE-DIMENSIONAL TRANSPORT, AND INVERSE GEOCHEMICAL CALCULATIONS, in Water resources investigations report 99-4259. 1999, USGS: Denver, Colorado.
7. Van Iseghem, P. et al. GLASTAB and GLAMOR projects: Main Conclusions and Remaining Uncertainties. in this conference. 2005.
8. Ferrand, K. et al. Silica sorption on container corrosion products siderite and magnetite. in this conference. 2005.
9. Cachoir, C. et al. , Effect of alpha irradiation field on long-term corrosion rates of spent fuel. 2005, European Commission, Joint Research Center, ITU: Karlsruhe.
10. Spahiu, K., Cui, D., and Lundström, M., The fate of radiolytic oxidants during spent fuel dissolution in the presence of dissolved near field hydrogen. Radiochim. Acta, 2004. 92 p. 625629.
11. Lundström, T., Radiation Chemistry of Aqueous Solutions Related to Nuclear Reactor Systems and Spent Fuel Management. 2003, Linköping Univerity: Linköping, Sweden.
12. Rother, A., Lutze, W., and Schubert-Bischoff, P., Characterization of lanthanoid phases formed upon glass dissolution in salt solutions. Mater. Res. Soc. Symp. Proc., 1992. 257 p. 5764.
13. Grambow, B. et al. , Release of Rare Earth Elements and Uranium from Glass in Low pH High Saline Brines. Radiochimica Acta, 1991. 52/53: p. 501506.
14. Sattonnay, G. et al. , Alpha-radiolysis effects on UO2 alteration in water. Journal of Nuclear Materials, 2001. 288 p. 1119.
15. Diaz Arocas, P. et al. , Coprecipitation of mono-, di-, tri-, tetra- and hexavalent Ions with Na-polyuranates. Radiochimica Acta, 1996. 74 p. 5158.
16. Rousseau, G., Coprécipitation de Th, Eu, La et Ac avec UO2 comme phase d'accueil., in Ecole Doctorale STIM. 2002, Université de Nantes: Nantes.
17. Bruno, J. and Sandino, A., The thermodynamics and kinetics of coprecipitation and its effect on radionuclide solubility. Radiochimica Acta, 1988. 44/45: p. 1721.
18. Langmuir, D., Uranium Solution-Mineral Equilibria at low Temperatures with Applications to Sedimentary ore Deposits. Geochimica et Cosmochimica Acta, 1978. 42 p. 547569.
19. Grenthe, I., Fuger, J., Konings, R.J.M., Lemire, R.J., Muller, A.B., Nguyen-Trung, C., Wanner, H., Chemical thermodynamics of uranium. North-Holland, Amsterdam, 1992: p. 0–0.
20. Robit, V. et al. Assessment of the relevance of coffinite formation within the nearfield environment of spent nuclear fuel geological disposal. in this conference. 2005. Gent.
21. Rovira, M. et al. , Study of the Role of Magnetite in the Immobilisation of U(VI) by Reduction to U(IV) under the Presence of H2(G) In Hydrogen Carbonate Media., in Technical Report. 2003, SKB: Stockholm.
22. Lemmens, K., The effect of clay on the dissolution of nuclear waste glass. J. Nucl. Mat., 2001. 298 p. 1118.
23. Godon, N. and Vernaz, E., R7T7 nuclear waste glass behavior in moist clay: role of the clay mass/glass surface area ratio. Mater. Res. Soc. Symp. Proc. (1990), 176(Sci. Basis Nucl. Waste Manage. 13), 319-26 CODEN: MRSPDH; ISSN: 0272-9172: p. F.
24. Grambow, B. et al. , Sorption of Cs, Ni, Pb, Eu, Am, Cm, Ac, Tc, Th, Zr, and U(IV) on MX-80 bentonite: an experimental approach to assess model uncertainty. Migration-05, Avignon 2005, 2005.
25. Bradbury, M.H. and Baeyens, B., Modelling the sorption of Mn(II), Co(II), Ni(II), Zn(II), Cd(II), Eu(III), Am(III), Sn(IV), Th(IV), Np(V) and U(VI) on montmorillonite: Linear free energy relationships and estimates of surface binding constants for some selected heavy metals and actinides, in Geochimica et Cosmochimica Acta. 2005. p. 875.
26. Evolution phénoménologique du stockage géologique, in Dossier 2005 Argile. 2005, ANDRA.
27. Savage, D., Noy, D.J., and Mihara, M., Modelling The Interaction Of Bentonite With Hyperalkaline Fluids. Applied Geochemistry, 2002. 17 p. 207223.
28. Gaucher, E. et al. , Modeling diffusion of an alkaline plume in a clay barrier. Applied Geochemistry, 2004. 19 p. 15051515.
29. ANDRA, Référentiel du comportement des radionucléides et des toxiques chimiques d'un stockage dans le Callovo-Oxfordien jusqu'à l'homme. Site de Meuse / Haute-Marne. 2005, ANDRA: Chatenay-Malabry.
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